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Corrosion-induced gas generation in a nuclear waste repository: Reactive geochemistry and multiphase flow effects
Authors:Tianfu Xu  Rainer Senger  Stefan Finsterle
Institution:aEarth Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA;bINTERA Inc., 1812 Centre Creek Drive, Suite 300, Austin, TX 78754, USA
Abstract:Corrosion of steel canisters, stored in a repository for spent fuel and high-level nuclear wastes, leads to the generation and accumulation of H2 gas in the backfilled emplacement tunnels, which may significantly affect long-term repository safety. Previous studies have used H2 generation rates based on the volume of the waste or canister material and the stoichiometry of the corrosion reaction. However, Fe corrosion and H2 generation rates vary with time, depending on factors such as amount of Fe, water availability, water contact area and aqueous and solid chemistry. To account for these factors and feedback mechanisms, a chemistry model was developed related to Fe corrosion, coupled with two-phase (liquid and gas) flow phenomena that are driven by gas-pressure buildup associated with H2 generation and water consumption. Results indicate that by dynamically calculating H2 generation rates based on a simple model of corrosion chemistry, and by coupling this corrosion reaction with two-phase flow processes, the degree and extent of gas-pressure buildup could be much smaller compared to a model that neglects the coupling between flow and reactive transport mechanisms. By considering the feedback of corrosion chemistry, the gas pressure increases initially at the canister, but later decreases and eventually returns to a stabilized pressure that is slightly higher than the background pressure. The current study focuses on corrosion under anaerobic conditions for which the coupled hydrogeochemical model was used to examine the role of selected physical parameters on H2 gas generation and corresponding pressure buildup in a nuclear waste repository. The developed model can be applied to evaluate the effect of water and mineral chemistry of the buffer and host rock on the corrosion reaction for future site-specific studies.
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